DOI: 10.1073/pnas.1612106114. Full atomistic reaction mechanism with kinetics for CO reduction on Cu(100) from ab initio molecular dynamics free-energy calculations at 298 K

Full atomistic reaction mechanism with kinetics for CO reduction on Cu(100) from ab initio molecular dynamics free-energy calculations at 298 K

10.1073/pnas.1612106114

Crossref journal-article

Proceedings of the National Academy of Sciences

Proceedings of the National Academy of Sciences (341)

Abstract

Significance Converting CO 2 to fuels is of great interest nowadays. Copper (Cu) is the only metal that produces hydrocarbon products, making it of interest for learning the reaction mechanisms underlying the selectivity and activity of Cu catalysts. In this report, we examine the reaction mechanism of CO reduction on Cu(100) at pH 7 including explicitly the aqueous solvent with ab initio molecular metadynamics simulations (AIMμD) free-energy calculations, which we find to explain all experimental observations. We expect that this understanding will suggest how to modify the Cu catalyst or replace it with a new material to enhance production of just a single such product while reducing the energy requirements (overpotential).

Bibliography

Cheng, T., Xiao, H., & Goddard, W. A. (2017). Full atomistic reaction mechanism with kinetics for CO reduction on Cu(100) from ab initio molecular dynamics free-energy calculations at 298 K. Proceedings of the National Academy of Sciences, 114(8), 1795â1800.

Authors 3

Tao Cheng (first)
Hai Xiao (additional)
William A. Goddard (additional)

References 50 Referenced 545

Dates

Type	When
Created	8 years, 6 months ago (Feb. 6, 2017, 9:05 p.m.)
Deposited	3 years, 4 months ago (April 13, 2022, 1:38 a.m.)
Indexed	1 day, 19 hours ago (Aug. 28, 2025, 8:03 a.m.)
Issued	8 years, 6 months ago (Feb. 6, 2017)
Published	8 years, 6 months ago (Feb. 6, 2017)
Published Online	8 years, 6 months ago (Feb. 6, 2017)
Published Print	8 years, 6 months ago (Feb. 21, 2017)

Funders 1

U.S. Department of Energy 10.13039/100000015
Region: Americas
gov (National government)
Labels8
1. Energy Department
2. Department of Energy
3. United States Department of Energy
4. ENERGY.GOV
5. US Department of Energy
6. USDOE
7. DOE
8. USADOE
Awards1
1. DE-SC0004993

BibTeX

@article{Cheng_2017, title={Full atomistic reaction mechanism with kinetics for CO reduction on Cu(100) from ab initio molecular dynamics free-energy calculations at 298 K}, volume={114}, ISSN={1091-6490}, url={http://dx.doi.org/10.1073/pnas.1612106114}, DOI={10.1073/pnas.1612106114}, number={8}, journal={Proceedings of the National Academy of Sciences}, publisher={Proceedings of the National Academy of Sciences}, author={Cheng, Tao and Xiao, Hai and Goddard, William A.}, year={2017}, month=feb, pages={1795–1800} }

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